In an attempt to reuse fibrous textile waste and, at the same time, to address dye pollution in textile wastewater, waste cotton-based yarn was utilized as both a cheap and sustainable adsorbent and a precursor for carbon adsorbent production. Cotton and cotton/polyester yarn samples underwent thermal modification through carbonization followed by chemical activation with KOH. Various techniques including nitrogen adsorption-desorption isotherms, scanning electron microscopy, Fourier transform infrared spectroscopy, and surface charge determination were employed to analyze the morphological and surface properties of the cotton-based adsorbents. Adsorption properties were evaluated by testing the removal of selected cationic and anionic dyes from water. The impact of temperature, contact time, initial concentration, and pH of the adsorbate solution on adsorption was investigated, with experimental data analyzed using theoretical models. While carbonization alone did not significantly enhance adsorption properties, activated samples exhibited high efficacy in removing both cationic and anionic dyes from water. Despite the negative influence of the polyester component in the carbon precursor on the efficiency of activated samples in removing methyl orange, results indicated that activated cotton and cotton/polyester yarn could be used to prepare highly efficient adsorbents for the rapid removal of methylene blue from real wastewater samples.